CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Hanzi Liu,Changfu You,Haiming Wang
Transient in-situ IR spectroscopy was performed to analyze the molecular behavior of selective catalytic reduction of NO with NH 3 on V 2 O 5 -WO 3 /TiO 2 catalyst. During NH 3 adsorption, an unexpected growth in the intensity of Lewis acid sites was observed due to the hydrogen migration, which was verified by the DFT calculation and the existence of intermediate species. The comparison between the isolated atmosphere experiments and the simultaneous exposure of NH 3 -NO-O 2 on catalytic monolayer demonstrated that: (i) there exists a pathway for Lewis to Brønsted acid sites transformation at T > 300 °C, (ii) the rate determining step of the SCR cycle involves in the re-oxidation of acid sites by O 2 at 200–300 °C. Generally, the Lewis acids are crucial at high temperatures, while Brønsted acids dominate the overall reaction at lower temperatures. Based on the experimental data and the DFT calculation, a mechanism for ammonia adsorption, acidity conversion and re-oxidation for the redox loop of the de-NOx reaction was proposed. The findings shed light on the understanding of relative strength of NO reduction and acid re-oxidation at different temperatures.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tianyun Zhao,Qiuwan Shen,Martin Andersson,Shian Li,Jinliang Yuan
High-entropy perovskite catalyst was synthesized and utilized for the first time in the MSR catalytic reaction. Among the HEPs, La(CoCuFeAlCe) 0.2 O 3 exhibited excellent MSR activity and high selectivity. The mechanism of the MSR reaction on the catalyst (100) surface was studied by employing DFT. The results indicate that the surface of La(CoCuFeAlCe) 0.2 O 3 catalyst has the lowest energy barrier, where the aldehyde hydrogenation reaction is the rate-determining step, explaining its high activity and selectivity. This research contributes additional evidence for the creation of high-entropy perovskite catalysts for MSR.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Sawsan Dacrory
3D multifunctional scaffold has been designed based on Cs/SA/NS/NPHA. Nanoparticles hydroxyapatite (NPHA) was prepared via precipitation method of sodium dihydrogen phosphate in presence calcium chloride . Different ratios of Chitosan (CS)/Sodium Alginate (SA) were used to prepare Cs/SA scaffolds in presence of CaCl 2 as a cross linker . NPHA was incorporated in CS/SA scaffold and neomycin sulfate (NS) was added as an antimicrobial agent. The structure and surface morphology of the scaffolds were investigated via infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM) and thermal gravimetric analysis (TGA) techniques. Additionally, Antimicrobial activity of the scaffold has evaluated against Gram- negative and Gram- positive bacteria. The result showed promising antimicrobial activity against Bacillus subtilis , Staphylococcus aureus , Escherichia coli , Pseudomonas aeruginosa and Candida albicans . Furthermore, cytotoxicity against MG63 osteosarcoma cell and fibroblast normal cell line has investigated. The result showed anti-proliferative against MG63. DFT calculations and molecular docking were used to study the reactivity of the compounds. The results exhibited that Cs/SA/NS/NPHA is potent expected to be used in bone tissue regeneration .
研究领域:
生物材料学
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药理学
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组织工程学
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Kun Yu,Huiting Li,Yiyi Yuan,Chenjia Ma,Bing Li,Jianzhong Guo
Superabsorbent hydrogels achieve the functional integration of water storage and fertilizer release through molecular design, offering an innovative pathway for the development of sustainable agricultural materials. Bamboo is a rapidly growing and widely distributed renewable biomass resource, and composite hydrogels with multiple functions can be constructed based on bamboo powder. This study developed a bio-based multifunctional superabsorbent hydrogel (BP-AD) that features both water retention and intelligent fertilizer control functions by grafting bamboo power (BP) with diacetone acrylamide (DAAM) and acrylic acid (AA) through an ultrasonic-assisted green aqueous solution polymerization technique. Characterization of FT-IR, XRD, and TGA confirmed that BP-AD is functionalized with carboxylic acid and amide groups and endows the material with excellent thermal stability. BP-AD exhibited an exceptional water absorbency capacity of 1401.5 g·g −1 in ultrapure water, and its water absorption kinetics followed the pseudo-second-order kinetic model (R 2 = 0.9991), indicating that chemical adsorption predominates in the moisture capture process. The adsorption of urea by BP-AD conforms to the Freundlich model, suggesting that multiphase multilayer adsorption is the mechanism behind urea adsorption. Density Functional Theory (DFT) calculations indicate that the adsorption of urea by BP-AD can be attributed to hydrogen bonding and electrostatic interactions. The release of urea from BP-AD aligns with both the Korsmeyer-Peppas model and Zero-order kinetic model, and regulated by an ionic strength response mechanism. This research integrates biomass resource conversion with precision modern agriculture by innovatively developing dual-functional hydrogels, offering technical support for sustainable agriculture.
研究领域:
材料科学
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农业工程
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高分子化学
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环境科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Chenxi Li,Yadan Guo,Dandan Tang,Yaoping Guo,Guanghui Wang,Hao Jiang,Jun Li
The density functional theory (DFT) not only is indispensable to calculate the electronic structure and chemical property of photocatalysts, but also provides guidance to the understanding of the mechanisms involved in photocatalysis. Herein, a novel Zn doped AgFeO 2 was successfully constructed for enhancement of Cr(VI) reduction and azophloxine decomposition under visible light irradiation. The DFT calculation was employed to set up a Zn doped AgFeO 2 model to simulate its split Zn 3 d levels shift to lower energy to optimize the band structure. With Zn doped, the AgFeO 2 exhibit enhanced reducing capacity. As expected, compared to unmodified AgFeO 2 , Zn doped AgFeO 2 can reduce and remove more than 90% of Cr(VI). Based on theoretical analysis and systematic experiments, the enhanced photocatalytic of Zn doped AgFeO 2 were arisen from superoxide radical (O 2 − ) generation and photocarrier transfer via oxygen vacancies (OVs) enrichment, and the OVs would provide coordinatively unsaturated sites for Cr(VI) adsorption. We expect this work can provide new insights into the photocatalytic utilization of AgFeO 2 .
研究领域:
材料科学
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环境科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mingjia Zhang,Fanyu Meng,Shule Zhang,Yiqing Zeng,Qin Zhong
The peroxone reaction between O 3 and H 2 O 2 over TiO 2 exhibits bright prospects for low-temperature flue gas denitration, which effectively overcomes the limitations of traditional peroxone reaction and remains advanced poison resistant ability. In this study, sulfur-doped TiO 2 was successfully adopted to improve the catalytic performance under low consumption of O 3 and H 2 O 2 , making this technology take a pivotal step towards practical application. Compared with TiO 2 /H 2 O 2 /O 3 system (68% NO conversion), the NO conversion could reach up to 85% in S-doped TiO 2 /H 2 O 2 /O 3 system under test condition (GHSV = 1.2 × 10 5 h −1 , H 2 O 2 /NO = 1.2, and O 3 /NO = 0.5). Characterizations and density functional theory calculations revealed that sulfur-doping modified the local structure of the catalyst, which enables a more effective combination between Ti 5c and hydroperoxyl, thus facilitating the reaction. Besides, the introduction of sulfur could increase the adsorption capacity of NO x and enhance the Lewis acidity of the catalyst, thus improving the NO conversion performance. The stability and applicability of the process were systematically tested from the following aspects: varied gas composition, H 2 O 2 consumption, pH value, and SO 2 /CO concentration. Results revealed that the S-doped TiO 2 /H 2 O 2 /O 3 system exhibited good stability and poison resistant ability, the potential for practical applications.
研究领域:
环境科学
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催化
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化学工程
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材料科学
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计算化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Yuanjing Du,Huinan Che,Peifang Wang,Juan Chen,Yanhui Ao
A novel carbon nitride based self-cleaning hydrogel photocatalyst (KI-PCN gel, potassium and iodine co-doped carbon nitride confined in alginate) has been successfully constructed by a facile method. Fabricated photocatalyst showed enhanced synergistic adsorption-photocatalytic degradation property on a high concentration of methylene blue (HMB) because of enhanced carrier separation efficiency and improved light adsorption capacity of KI-PCN. As expected, the KI-PCN gel showed the highest apparent rate constant value ( K app =0.0310 min −1 ), which was about 38.8 and 5.8 times as that of blank hydrogel ( K app =0.0008 min −1 ) and PCN gel ( K app =0.0053 min −1 ), respectively. Meanwhile, KI-PCN gel can continuously adsorb low concentration of MB (LMB), and the MB-adsorbed KI-PCN gel can self-clean under light irradiation. The bench-scale experiments simulating real river showed that KI-PCN gel can effectively and continuously remove LMB (0.1–20 ppm), indicating the possibility for the removal of contaminants in natural rivers. Furthermore, the possible degradation pathways were proposed by combining the density functional calculations (DFT) and intermediates identified by liquid chromatography-mass spectrometry (LC-MS). This work proposed a new perspective to acquire a novel self-cleaning and easily recyclable photocatalyst for treatment of wide concentration range organic wastewater as well as remediation of natural waterbody.
研究领域:
环境科学
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材料科学
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化学
·
水处理
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DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 61
·37014-37022
·
IF 3.119
Shengfu Liao,Jianguo Liu,Long Yan,Qiying Liu,Guanghui Chen,Longlong Ma
Anthraquinones are recognized as high efficiency photocatalysts which can perform various redox reactions in aqueous or organic phases. We have experimentally proven that 2-BrAQ can undergo hydrogen transfer with an alpha-aromatic alcohol under light conditions, thereby efficiently oxidizing the aromatic alcohol to the corresponding product. The yield of 1-phenethanol to acetophenone can reach more than 96%. In subsequent catalyst screening experiments, it was found that the electronegativity of the substituent at the 2 position of the anthraquinone ring and the acidity of the solvent affect the photocatalytic activity of anthraquinones. After using various aromatic alcohol substrates, 2-BrAQ showed good conversion and selectivity for most aromatic alcohols, but showed C–C bond cleavage and low selectivity with non-α-position aromatic alcohols. In order to explore the mechanism of the redox reaction of 2-BrAQ in acetonitrile solution, the corresponding free radical reaction pathway was proposed and verified by density functional theory (DFT). Focusing on calculations for 2-BrAQ during the reaction and the first-step hydrogen transfer reaction between the 2-BrAQ triplet molecule and the 1-phenylethanol molecule, we recognized the changes that occurred during the reaction and thus have a deeper understanding of the redox reaction of anthraquinone compounds in organic systems.
研究领域:
化学
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催化
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有机化学
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理论化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Toxics
·
2024
·Vol. 12
·期 1
·43
·
IF 3.9
Mingguo Peng,Yang Xu,Yao Wu,Xuewen Cai,Weihua Zhang,Lu Zheng,Erdeng Du,Jiajun Fu
Per- and Polyfluoroalkyl Substances (PFAS) bioaccumulate in the human body, presenting potential health risks and cellular toxicity. Their transport mechanisms and interactions with tissues and the circulatory system require further investigation. This study investigates the interaction mechanisms of six PFAS with Human Serum Albumin (HSA) using multi-spectroscopy, DFT and a molecular dynamics approach. Multi-spectral analysis shows that perfluorononanoic acid (PFNA) has the best binding capabilities with HSA. The order of binding constants (298 K) is as follows: “Perfluorononanoic Acid (PFNA, 7.81 × 106L·mol−1) > Perfluoro-2,5-dimethyl-3,6-dioxanonanoic Acid (HFPO-TA, 3.70 × 106L·mol−1) > Perfluorooctanoic Acid (PFOA, 2.27 × 105L·mol−1) > Perfluoro-3,6,9-trioxadecanoic Acid (PFO3DA, 1.59 × 105L·mol−1) > Perfluoroheptanoic Acid (PFHpA, 4.53 × 103L·mol−1) > Dodecafluorosuberic Acid (DFSA, 1.52 × 103L·mol−1)”. Thermodynamic analysis suggests that PFNA and PFO3DA’s interactions with HSA are exothermic, driven primarily by hydrogen bonds or van der Waals interactions. PFHpA, DFSA, PFOA, and HFPO-TA’s interactions with HSA, on the other hand, are endothermic processes primarily driven by hydrophobic interactions. Competitive probe results show that the main HSA–PFAS binding site is in the HSA structure’s subdomain IIA. These findings are also consistent with the findings of molecular docking. Molecular dynamics simulation (MD) analysis further shows that the lowest binding energy (−38.83 kcal/mol) is fund in the HSA–PFNA complex, indicating that PFNA binds more readily with HSA. Energy decomposition analysis also indicates that van der Waals and electrostatic interactions are the main forces for the HSA–PFAS complexes. Correlation analysis reveals that DFT quantum chemical descriptors related to electrostatic distribution and characteristics like ESP and ALIE are more representative in characterizing HSA–PFAS binding. This study sheds light on the interactions between HSA and PFAS. It guides health risk assessments and control strategies against PFAS, serving as a critical starting point for further public health research.Keywords:human serum albumin (HSA);per- and polyfluoroalkyl substances (PFAS);multi-spectroscopy;DFT calculations;molecular docking;molecular dynamics simulation
研究领域:
生物化学
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环境科学
·
毒理学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 3
·1197-1208
·
IF 3.925
Wei-Ye Zhang,Si-Qing Ye,Xin-Tao Yang,Bao-Shi Zhu,Wei-Li Li,Hong-Xing He,Xiu-Jun Deng
A novel magnetic graphene oxide-based surface imprinted polymer (Fe3O4@GO@IIP) was synthesized using the surface imprinting technology to selectively adsorb Ni(II) from aqueous solution. The imprinted polymer was characterized by FT-IR, XRD, SEM, TEM, VSM, TGA and XPS. The results showed that the sorbent exhibited good thermal and mechanical stability, and can be quickly separated from the solution by applying an external magnetic field. The adsorption performance indicated that the prepared imprinted material had a short adsorption equilibrium time (16 min) and a high adsorption capacity (35.31 mg g−1) for Ni(II) at an optimal pH of 6.0. The selectivity coefficients of the imprinted material were 17.57, 16.27, 10.86, 14.27 and 17.65 for Ni(II)/Co(II), Ni(II)/Cu(II), Ni(II)/Pb(II) Ni(II)/Cd(II), and Ni(II)/Zn(II), respectively. Reusability studies indicated that the adsorption capacity of the prepared polymer did not decrease significantly after repeated use ten times. Moreover, the adsorption mechanism of Ni(II) by the imprinted polymer was also studied. The adsorption process was spontaneous and endothermic, and followed the pseudo-secondary kinetic model and the Langmuir model. The results of the Scatchard model indicated the presence of two Ni(II) strong binding sites on Fe3O4@GO@IIP, where the single-bond O atom of the sulfonic acid group and the N atom of the –N–CO group in AMPS played a dominant role in Ni(II) adsorption, as conformed by both DFT calculations and XPS.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS
·
2019
·
IF 3.31
Yu-Jie Luo,Bao-Li Wang,Song-Bo Kou,Zhen-Yi Lin,Kai-Li Zhou,Yan-Yue Lou,Jie-Hua Shi
The binding characteristics of calf thymus DNA (ct-DNA) with dasatinib (DSTN), a tyrosine kinase inhibitor was assessed through multi-spectroscopic methodologies and viscosity measurement combined with molecular docking as well as DFT calculation to understand the binding mechanism, affinity of DSTN onto ct-DNA, effect of DSTN on ct-DNA conformation, and among others. The results confirmed DSTN bound onto ct-DNA, leading to forming the DSTN–ct-DNA complex with the binding constant of 4.82 × 103 M−1 at 310 K. DSTN preferentially inserted to the minor groove of ct-DNA with rich A-T region, that was the binding mode of DSTN onto ct-DNA was groove binding. The enthalpic change (ΔH0) and entropic change (ΔS0) during the binding process of DSTN with ct-DNA were 128.9 kJ mol−1 and 489.2 J mol−1 K−1, respectively, confirming clearly that the association of DSTN with ct-DNA was an endothermic process and the dominative driven-force was hydrophobic interaction. Meanwhile, the results also indicated that there was a certain extent of electrostatic force and hydrogen bonding, but they maybe play an auxiliary role. The CD measurement results confirmed the alteration in the helical configuration of ct-DNA but almost no change in the base stacking after binding DSTN. The results revealed that there was the obvious change in the conformation, the dipole moment, and the atomic charge distribution of DSTN in the B-DNA complexes, compared with free DSTN, to satisfy the conformational adaptation. From the obtained fronitier molecular orbitals of DSTN, it can be inferred that the nature of DSTN alters with the change of the environment around DSTN.Communicated by Ramaswamy H. Sarma
研究领域:
生物化学
·
药物化学
·
分子生物学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Hainan Wei,Fanming Meng,Han Zhang,Wenqing Yu,Jialong Li,Sheng Yao
Constructing new photocatalysts for the photocatalytic reduction of CO 2 and efficient degradation of Levofloxacin is of great importance to renewable energy. Here, S-scheme Bi 2 MoO 6- x /MoS 2 heterojunction nanospheres containing abundant surface defects (oxygen vacancies) were designed and successfully synthesized to enhance CO 2 photoreduction activity in the absence of other sacrificial agents, co-catalysts or photosensitisers. At the same time, it can efficiently degrade organic pollutants (Levofloxacin). This heterogeneous structure with surface defects provides an abundance of reactive sites, accelerates charge separation and improves oxidation capacity. The improved Bi 2 MoO 6- x /MoS 2 heterogeneous nanospheres show excellent performance under simulated solar light, with the selectivity and yield of 92.45% and 29.01 µmol h −1 , respectively, for the generation of CO. Under visible light, the degradation efficiency of levofloxacin hydrochloride (LVX) reached 96.3% within 25 min and remained as high as 95% after three cycles. This work provides a new idea for the design of new S-scheme photocatalysts and an important reference for the preparation of photocatalysts for the efficient photocatalytic reduction of CO 2 and the efficient degradation of organic pollutants at the same time.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）